Facile synthesis of hierarchical flower-like Ag/Cu2O and Au/Cu2O nanostructures and enhanced catalytic performance in electrochemical reduction of CO2

Mengyun Wang, Shengbo Zhang, Mei Li, Aiguo Han, Xinli Zhu, Qingfeng Ge, Jinyu Han, Hua Wang

PDF(3476 KB)
PDF(3476 KB)
Front. Chem. Sci. Eng. ›› 2020, Vol. 14 ›› Issue (5) : 813-823. DOI: 10.1007/s11705-019-1854-8
RESEARCH ARTICLE
RESEARCH ARTICLE

Facile synthesis of hierarchical flower-like Ag/Cu2O and Au/Cu2O nanostructures and enhanced catalytic performance in electrochemical reduction of CO2

Author information +
History +

Abstract

Novel, hierarchical, flower-like Ag/Cu2O and Au/Cu2O nanostructures were successfully fabricated and applied as efficient electrocatalysts for the electrochemical reduction of CO2. Cu2O nanospheres with a uniform size of ~180 nm were initially synthesized. Thereafter, Cu2O was used as a sacrificial template to prepare a series of Ag/Cu2O composites through galvanic replacement. By varying the Ag/Cu atomic ratio, Ag0.125/Cu2O, having a hierarchical, flower-like nanostructure with intersecting Ag nanoflakes encompassing an inner Cu2O sphere, was prepared. The as-prepared Agx/Cu2O samples presented higher Faradaic efficiencies (FE) for CO and relatively suppressed H2 evolution than the parent Cu2O nanospheres due to the combination of Ag with Cu2O in the former. Notably, the highest CO evolution rate was achieved with Ag0.125/Cu2O due to the larger electroactive surface area furnished by the hierarchical structure. The same hierarchical flower-like structure was also obtained for the Au0.6/Cu2O composite, where the FECO (10%) was even higher than that of Ag0.125/Cu2O. Importantly, the results reveal that Ag0.125/Cu2O and Au0.6/Cu2O both exhibit remarkably improved stability relative to Cu2O. This study presents a facile method of developing hierarchical metal-oxide composites as efficient and stable electrocatalysts for the electrochemical reduction of CO2.

Keywords

bimetallic nanostructure / hierarchical metal/oxide nanomaterial / galvanic replacement / electrochemical reduction of CO2

Cite this article

Download citation ▾
Mengyun Wang, Shengbo Zhang, Mei Li, Aiguo Han, Xinli Zhu, Qingfeng Ge, Jinyu Han, Hua Wang. Facile synthesis of hierarchical flower-like Ag/Cu2O and Au/Cu2O nanostructures and enhanced catalytic performance in electrochemical reduction of CO2. Front. Chem. Sci. Eng., 2020, 14(5): 813‒823 https://doi.org/10.1007/s11705-019-1854-8

References

[1]
Jin Z, Li P, Liu G, Zheng B, Yuan H, Xiao D. Enhancing catalytic formaldehyde oxidation on CuO–Ag2O nanowires for gas sensing and hydrogen evolution. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 2013, 1(46): 14736–14743
CrossRef Google scholar
[2]
Park J, Liu J, Peng H, Figueroa-Cosme L, Miao S, Choi S, Bao S, Yang X, Xia Y. Coating Pt–Ni octahedra with ultrathin Pt shells to enhance the durability without compromising the activity toward oxygen reduction. ChemSusChem, 2016, 9(16): 2209–2215
CrossRef Google scholar
[3]
Liu H, Koenigsmann C, Adzic R R, Wong S S. Probing ultrathin one-dimensional Pd-Ni nanostructures as oxygen reduction reaction catalysts. ACS Catalysis, 2014, 4(8): 2544–2555
CrossRef Google scholar
[4]
Wang Y, Zhang J. Structural engineering of transition metal-based nanostructured electrocatalysts for efficient water splitting. Frontiers of Chemical Science and Engineering, 2018, 12(4): 838–854
CrossRef Google scholar
[5]
Qu X, Yang R, Tong F, Zhao Y, Wang M. Hierarchical ZnO microstructures decorated with Au nanoparticles for enhanced gas sensing and photocatalytic properties. Powder Technology, 2018, 330: 259–265
CrossRef Google scholar
[6]
Su Y, Guo H, Wang Z, Long Y, Li W, Tu Y. Au@Cu2O core-shell structure for high sensitive non-enzymatic glucose sensor. Sensors and Actuators. B, Chemical, 2018, 255: 2510–2519
CrossRef Google scholar
[7]
Pang M, Wang Q, Zeng H C. Self-Generated etchant for synthetic sculpturing of Cu2O-Au, Cu2O@Au, Au/Cu2O, and 3D-Au Nanostructures. Chemistry (Weinheim an der Bergstrasse, Germany), 2012, 18(46): 14605–14609
CrossRef Google scholar
[8]
Rodrigues T S, Da Silva A G M, Alves R S, de Freitas I C, Oliveira D C, Camargo P H C. Controlling reduction kinetics in the galvanic replacement involving metal oxides templates: Elucidating the formation of bimetallic bowls, rattles, and dendrites from Cu2O Spheres. Particle & Particle Systems Characterization, 2018, 35(5): 1700175–1700184
CrossRef Google scholar
[9]
Zhu H, Du M, Yu D, Wang Y, Zou M, Xu C, Fu Y. Selective growth of Au nanograins on specific positions (tips, edges and facets) of Cu2O octahedrons to form Cu2O–Au hierarchical heterostructures. Dalton Transactions (Cambridge, England), 2012, 41(45): 13795–13799
CrossRef Google scholar
[10]
Polavarapu L, Zanaga D, Altantzis T, Rodal-Cedeira S, Pastoriza-Santos I, Pérez-Juste J, Bals S, Liz-Marzán L M. Galvanic replacement coupled to seeded growth as a route for shape-controlled synthesis of plasmonic nanorattles. Journal of the American Chemical Society, 2016, 138(36): 11453–11456
CrossRef Google scholar
[11]
Zhu H, Du M L, Yu D L, Wang Y, Wang L N, Zou M L, Zhang M, Fu Y. A new strategy for the surface-free-energy-distribution induced selective growth and controlled formation of Cu2O–Au hierarchical heterostructures with a series of morphological evolutions. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 2013, 1(3): 919–929
CrossRef Google scholar
[12]
Zhang Y, Zhou X, Zhao Y, Liu Z, Ma D, Chen S, Zhu G, Li X. One-step solvothermal synthesis of interlaced nanoflake-assembled flower-like hierarchical Ag/Cu2O composite microspheres with enhanced visible light photocatalytic properties. Royal Society of Chemistry Advances, 2017, 7(12): 6957–6965
CrossRef Google scholar
[13]
Wang J, Wang H, Han Z, Han J. Electrodeposited porous Pb electrode with improved electrocatalytic performance for the electroreduction of CO2 to formic acid. Frontiers of Chemical Science and Engineering, 2015, 9(1): 57–63
CrossRef Google scholar
[14]
Song G, Wu X, Xin F, Yin X. ZnFe2O4 deposited on BiOCl with exposed (001) and (010) facets for photocatalytic reduction of CO2 in cyclohexanol. Frontiers of Chemical Science and Engineering, 2017, 11(2): 197–204
CrossRef Google scholar
[15]
Xie H, Wang J, Ithisuphalap K, Wu G, Li Q. Recent advances in Cu-based nanocomposite photocatalysts for CO2 conversion to solar fuels. Journal of Energy Chemistry, 2017, 26(6): 1039–1049
CrossRef Google scholar
[16]
Qin T, Qian Y, Zhang F, Lin B. Cloride-derived copper electrode for efficient electrochemical reduction of CO2 to ethylene. Chinese Chemical Letters, 2019, 30(2): 314–318
CrossRef Google scholar
[17]
He J, Johnson N J J, Huang A, Berlinguette C P. Electrocatalytic alloys for CO2 reduction. ChemSusChem, 2018, 11(1): 48–57
CrossRef Google scholar
[18]
Singh S, Gautam R K, Malik K, Verma A. Ag-Co bimetallic catalyst for electrochemical reduction of CO2 to value added products. Journal of CO2 Utilization, 2017, 18: 139–146
[19]
Kim D, Resasco J, Yu Y, Asiri A M, Yang P. Synergistic geometric and electronic effects for electrochemical reduction of carbon dioxide using gold–copper bimetallic nanoparticles. Nature Communications, 2014, 5(1): 5948–5956
CrossRef Google scholar
[20]
Yang J, Liu X, Cao H, Shi Y, Xie Y, Xiao J. Dendritic BiVO4 decorated with MnOx co-catalyst as an efficient hierarchical catalyst for photocatalytic ozonation. Frontiers of Chemical Science and Engineering, 2019, 13(1): 185–191
CrossRef Google scholar
[21]
Zhang B, Zhang J. Rational design of Cu-based electrocatalysts for electrochemical reduction of carbon dioxide. Journal of Energy Chemistry, 2017, 26(6): 1050–1066
CrossRef Google scholar
[22]
Kim J, Woo H, Yun S, Jung H, Back S, Jung Y, Kim Y. Highly active and selective Au thin layer on Cu polycrystalline surface prepared by galvanic displacement for the electrochemical reduction of CO2 to CO. Applied Catalysis B: Environmental, 2017, 213: 211–215
CrossRef Google scholar
[23]
Kuo M, Hsiao C, Chiu Y, Lai T, Fang M, Wu J, Chen J, Wu C, Wei K, Lin H, Hsu Y. Au@Cu2O core@shell nanocrystals as dual-functional catalysts for sustainable environmental applications. Applied Catalysis B: Environmental, 2019, 242: 499–506
CrossRef Google scholar
[24]
Lee S, Park G, Lee J. Importance of Ag-Cu biphasic boundaries for selective electrochemical reduction of CO2 to ethanol. ACS Catalysis, 2017, 7(12): 8594–8604
CrossRef Google scholar
[25]
Jin W, Xu P, Xiong L, Jing Q, Zhang B, Sun K, Han X. SERS-active silver nanoparticle assemblies on branched Cu2O crystals through controlled galvanic replacement. Royal Society of Chemistry Advances, 2014, 4(96): 53543–53546
CrossRef Google scholar
[26]
Chen S, Liu P, Su K, Li X, Qin Z, Xu W, Chen J, Li C, Qiu J. Electrochemical aptasensor for thrombin using co-catalysis of hemin/Gquadruplex DNAzyme and octahedral Cu2O-Au nanocomposites for signal amplification. Biosensors & Bioelectronics, 2018, 99: 338–345
CrossRef Google scholar
[27]
Dai D, Liu H, Ma H, Huang Z, Gu C, Zhang M. In-situ synthesis of Cu2O-Au nanocomposites as nanozyme for colorimetric determination of hydrogen peroxide. Journal of Alloys and Compounds, 2018, 747: 676–683
CrossRef Google scholar
[28]
Luo H, Zhou J, Zhong H, Zhou L, Jia Z, Tan X. Polyhedron Cu2O@Ag composite microstructures: Synthesis, mechanism analysis and structure dependent SERS properties. Royal Society of Chemistry Advances, 2016, 6(101): 99105–99113
CrossRef Google scholar
[29]
Kandula S, Jeevanandam P. Synthesis of Cu2O@Ag polyhedral core–shell nanoparticles by a thermal decomposition approach for catalytic applications. European Journal of Inorganic Chemistry, 2016, 2016(10): 1548–1557
CrossRef Google scholar
[30]
Wang Y, Gao T, Wang K, Wu X, Shi X, Liu Y, Lou S, Zhou S. Template-assisted synthesis of uniform nanosheet-assembled silver hollow microcubes. Nanoscale, 2012, 4(22): 7121–7126
CrossRef Google scholar
[31]
Biesinger M C, Lau L W M, Gerson A R, Smart R S C. Resolving surface chemical states in XPS analysis of first row transition metals, oxides and hydroxides: Sc, Ti, V, Cu and Zn. Applied Surface Science, 2010, 257(3): 887–898
CrossRef Google scholar
[32]
Li C W, Kanan M W. CO2 reduction at low overpotential on Cu electrodes resulting from the reduction of thick Cu2O films. Journal of the American Chemical Society, 2012, 134(17): 7231–7234
CrossRef Google scholar
[33]
Raciti D, Livi K J, Wang C. Highly dense Cu nanowires for low-overpotential CO2 reduction. Nano Letters, 2015, 15(10): 6829–6835
CrossRef Google scholar

Acknowledgements

We are grateful to the Analysis and Test Center of Tianjin University for providing XRD, SEM, and TEM characterization. We also acknowledge the National Natural Science Foundation of China (Grant Nos. 21576204 and 21206117) for financial support.

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11705-019-1854-8 and is accessible for authorized users.

RIGHTS & PERMISSIONS

2019 Higher Education Press and Springer-Verlag GmbH Germany, part of Springer Nature
AI Summary AI Mindmap
PDF(3476 KB)

Accesses

Citations

Detail

Sections
Recommended

/